Treatment of [MoO(N-t-Bu)Cl-2(dme)] (dme = dimethoxyethane) with 2 equiv of the potassium salts of Schiff base ligands of the type KArNC(CH3)CHC(CH3)O afforded oxo imido molybdenum(VI) compounds [MoO(N-t-Bu)L-2] {1, with Ar = PhenYl (Lph), 2 with Ar = 2-tolyl (Wert), 3 with Ar = 2,6-dimethylphenyl (L-Me2Ph) and 4 with Ar = 2,6-diisopropylphenyl (L-ipr2Ph)} We have also prepared related bisimido complexes [Mo(N-t-Bu)(2)L-2 (5 with L=L-ph, 6 with L = L-meph, and 7 with L = L-Me2Ph) by treatment of [Mo(N-(-Bu)(2)Cl-2(dme)] with 2 equiv of the potassium salt of the respective ligand. 1, 3, 5, and 6 were characterized via single crystal X-ray diffraction. The oxo imido complexes exhibit oxygen atom transfer (OAT) reactivity toward trimethyl phosphine. Kinetic data were obtained for 1 and 3 by UV/vis spectroscopy revealing decreased OAT reactivity in comparison to related dioxo complexes with the same Schiff base ligands and decreased reactivity of 1 versus 3. Cyclic voltammetry was used to probe the electronic situation at the molybdenum center showing reversible reduction waves for 3 and [MoO2(L-me2Ph)2, 1 at comparable potentials while 1 exhibits a significant lower potential. Density functional theory (OFT) calculations showed a higher electron density on oxygen in the oxo imido compleges.